Pub Date : 2025-11-14DOI: 10.1016/j.joule.2025.102209
Ilhem Nadia Rabehi, Silvia Mariotti, Kenjiro Fukuda, Shin Young Lee, Dou Zhao, Penghui Ji, Shuai Yuan, Jiahao Zhang, Chenfeng Ding, Kirill Mitrofanov, Dominik Madea, Ryota Kabe, Tomoyuki Yokota, Luis K. Ono, Takao Someya, Yabing Qi
Perovskite materials are highly promising for ultra-flexible solar cells (u-FPSCs) due to their intrinsic mechanical flexibility and lightweight nature. Devices fabricated on substrates thinner than 10 μm are particularly attractive for emerging applications in wearable electronics and medical applications. Although their power conversion efficiency (PCE) approaches that of rigid glass-based devices, long-term stability remains a critical challenge. In this study, we show that the combination of nickel oxide and [2-(9H-carbazol-9-yl)ethyl]phosphonic acid (2PACz) self-assembled monolayer as hole transport materials employed on indium tin oxide-coated transparent polyimide leads to a significant improvement of the device stability. This strategy enabled devices with PCEs of 20.3% and a stable power output for 1,200 h under inert conditions. Furthermore, the integration of a 15-nm Al₂O₃ humidity barrier preserved 90% of the PCE after 130 h in air, without compromising specific power (27.2 W g−1), establishing record ambient stability for u-FPSCs.
钙钛矿材料由于其固有的机械灵活性和轻质性，在超柔性太阳能电池（u-FPSCs）中具有很高的应用前景。在厚度小于10 μm的基板上制造的器件对于可穿戴电子产品和医疗应用中的新兴应用尤其具有吸引力。虽然它们的功率转换效率（PCE）接近刚性玻璃基器件，但长期稳定性仍然是一个关键挑战。在本研究中，我们证明了将氧化镍和[2-（9h -咔唑-9-基）乙基]膦酸（2PACz）自组装单层作为空穴传输材料应用于氧化铟锡涂层的透明聚酰亚胺上，可以显著提高器件的稳定性。该策略使器件的pce为20.3%，在惰性条件下稳定输出功率为1200小时。此外，集成的15纳米Al₂O₃湿度屏障在空气中放置130小时后保留了90%的PCE，而不影响比功率（27.2 W g−1），为u-FPSCs建立了创纪录的环境稳定性。
{"title":"Dual hole transport layer for ultra-flexible perovskite solar cells with unprecedented stability","authors":"Ilhem Nadia Rabehi, Silvia Mariotti, Kenjiro Fukuda, Shin Young Lee, Dou Zhao, Penghui Ji, Shuai Yuan, Jiahao Zhang, Chenfeng Ding, Kirill Mitrofanov, Dominik Madea, Ryota Kabe, Tomoyuki Yokota, Luis K. Ono, Takao Someya, Yabing Qi","doi":"10.1016/j.joule.2025.102209","DOIUrl":"https://doi.org/10.1016/j.joule.2025.102209","url":null,"abstract":"Perovskite materials are highly promising for ultra-flexible solar cells (u-FPSCs) due to their intrinsic mechanical flexibility and lightweight nature. Devices fabricated on substrates thinner than 10 μm are particularly attractive for emerging applications in wearable electronics and medical applications. Although their power conversion efficiency (PCE) approaches that of rigid glass-based devices, long-term stability remains a critical challenge. In this study, we show that the combination of nickel oxide and [2-(9H-carbazol-9-yl)ethyl]phosphonic acid (2PACz) self-assembled monolayer as hole transport materials employed on indium tin oxide-coated transparent polyimide leads to a significant improvement of the device stability. This strategy enabled devices with PCEs of 20.3% and a stable power output for 1,200 h under inert conditions. Furthermore, the integration of a 15-nm Al₂O₃ humidity barrier preserved 90% of the PCE after 130 h in air, without compromising specific power (27.2 W g<sup>−1</sup>), establishing record ambient stability for u-FPSCs.","PeriodicalId":343,"journal":{"name":"Joule","volume":"19 1","pages":""},"PeriodicalIF":39.8,"publicationDate":"2025-11-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145509898","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-11-11DOI: 10.1016/j.joule.2025.102200
Tian (Leo) Jin, Pin Chen, Jingtao Wang, Yuan Yu, Yue Gong, Qiang Zheng, Tianxing Wang, Yutong Lu, Rongqian Wu, Jie Chen, Yi Lyu, Shaohua Shen, Xiaofei Liu
Developing non-noble metal-based chlorine evolution reaction (CER) catalysts to compete with noble metals-containing dimensionally stable anodes is challenging. Multi-metal oxides are promising for CER, but their discovery heavily depends on human-driven experimentation. Herein, an atomic-level entropy-guided strategy combining density functional theory (DFT) and data-driven machine learning (ML) was developed to accelerate the discovery of non-noble metal-based MSb2O6-type trirutile antimonates for CER. The high-entropy effect could benefit CER with excellent activity and stability by optimizing the electronic structure. High-entropy trirutile antimonates, with oxygen vacancies and lattice strain, reduce the energy barrier at Cu sites for Cl∗ adsorption, achieving a record-low overpotential of 24 mV at 10 mA cm−2, >95% faradaic efficiency, and 160-h stability at 50 mA cm−2. The presented atomic-level entropy-guided strategy would inspire the rational design of highly active and stable electrocatalysts for CER and other electrocatalysis applications.
开发非贵金属基氯析出反应（CER）催化剂以与含贵金属的尺寸稳定阳极竞争是一项具有挑战性的工作。多金属氧化物很有希望用于CER，但它们的发现在很大程度上取决于人类驱动的实验。本文提出了一种原子级熵引导策略，结合密度泛函理论（DFT）和数据驱动机器学习（ML），以加速发现非贵金属基msb2o6型三萜锑酸盐。高熵效应通过优化电子结构使CER具有良好的活性和稳定性。具有氧空位和晶格应变的高熵三维锑酸盐降低了Cu位上Cl *吸附的能垒，在10 mA cm−2下达到了创纪录的24 mV过电位，95%的法拉第效率和50 mA cm−2下160 h的稳定性。本文提出的原子能级熵导策略将为CER和其他电催化应用提供高效稳定的电催化剂的合理设计。
{"title":"Entropy-guided discovery of denary trirutile antimonates for electrocatalytic chlorine evolution","authors":"Tian (Leo) Jin, Pin Chen, Jingtao Wang, Yuan Yu, Yue Gong, Qiang Zheng, Tianxing Wang, Yutong Lu, Rongqian Wu, Jie Chen, Yi Lyu, Shaohua Shen, Xiaofei Liu","doi":"10.1016/j.joule.2025.102200","DOIUrl":"https://doi.org/10.1016/j.joule.2025.102200","url":null,"abstract":"Developing non-noble metal-based chlorine evolution reaction (CER) catalysts to compete with noble metals-containing dimensionally stable anodes is challenging. Multi-metal oxides are promising for CER, but their discovery heavily depends on human-driven experimentation. Herein, an atomic-level entropy-guided strategy combining density functional theory (DFT) and data-driven machine learning (ML) was developed to accelerate the discovery of non-noble metal-based MSb<sub>2</sub>O<sub>6</sub>-type trirutile antimonates for CER. The high-entropy effect could benefit CER with excellent activity and stability by optimizing the electronic structure. High-entropy trirutile antimonates, with oxygen vacancies and lattice strain, reduce the energy barrier at Cu sites for Cl∗ adsorption, achieving a record-low overpotential of 24 mV at 10 mA cm<sup>−2</sup>, >95% faradaic efficiency, and 160-h stability at 50 mA cm<sup>−2</sup>. The presented atomic-level entropy-guided strategy would inspire the rational design of highly active and stable electrocatalysts for CER and other electrocatalysis applications.","PeriodicalId":343,"journal":{"name":"Joule","volume":"28 1","pages":""},"PeriodicalIF":39.8,"publicationDate":"2025-11-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145485785","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
The performance of gas diffusion electrodes (GDEs) with high catalyst loadings for multiphase electrochemical conversion is often compromised by sluggish mass transport arising from competing gas-liquid transport through the tortuous pore structure. Inspired by ridge-furrow irrigation in agriculture, we propose an aligned-pore engineering strategy to decouple the competing transport processes by leveraging pore-size-dependent capillary forces and enrich abundant three-phase interfaces (TPIs) in GDEs. Compared with a conventional electrode, the engineered electrode has a 46% lower mass transport impedance and 1.96-fold more TPIs. The optimized electrode delivers a maximum power (current) density of 85.5 mW cm−2 (634.4 mA cm−2), which is 82% (83%) higher than that of the conventional electrode, standing out as the highest reported for air-breathing membraneless direct formate fuel cells (DFFCs). The universality of this strategy is validated for direct methanol fuel cells, zinc-air batteries, and CO2 electrolysis cells, demonstrating broad applicability for high-performance GDEs.
高催化剂负载的气体扩散电极（GDEs）的多相电化学转化性能经常受到通过弯曲孔隙结构的气液相互竞争所引起的缓慢的质量传递的影响。受农业垄沟灌溉的启发，我们提出了一种对齐孔工程策略，通过利用孔径依赖的毛细力和丰富的GDEs三相界面（tpi）来解耦竞争的运输过程。与传统电极相比，工程电极的质量传输阻抗降低了46%，tpi增加了1.96倍。优化后的电极提供的最大功率（电流）密度为85.5 mW cm - 2 (634.4 mA cm - 2)，比传统电极高82%(83%)，是目前报道的呼吸式无膜直接甲酸盐燃料电池（DFFCs）中最高的。该策略的通用性在直接甲醇燃料电池、锌空气电池和二氧化碳电解电池中得到了验证，证明了高性能gde的广泛适用性。
{"title":"Aligned-pore engineering: Decoupling gas-liquid transport in gas diffusion electrodes","authors":"Qin Peng, Haokai Xu, Yuan He, Yutong Jiang, Zhenglong Wu, Yudong Zhang, Xun Zhu, Jun Li, Wei Yang, Qiang Liao","doi":"10.1016/j.joule.2025.102199","DOIUrl":"https://doi.org/10.1016/j.joule.2025.102199","url":null,"abstract":"The performance of gas diffusion electrodes (GDEs) with high catalyst loadings for multiphase electrochemical conversion is often compromised by sluggish mass transport arising from competing gas-liquid transport through the tortuous pore structure. Inspired by ridge-furrow irrigation in agriculture, we propose an aligned-pore engineering strategy to decouple the competing transport processes by leveraging pore-size-dependent capillary forces and enrich abundant three-phase interfaces (TPIs) in GDEs. Compared with a conventional electrode, the engineered electrode has a 46% lower mass transport impedance and 1.96-fold more TPIs. The optimized electrode delivers a maximum power (current) density of 85.5 mW cm<sup>−2</sup> (634.4 mA cm<sup>−2</sup>), which is 82% (83%) higher than that of the conventional electrode, standing out as the highest reported for air-breathing membraneless direct formate fuel cells (DFFCs). The universality of this strategy is validated for direct methanol fuel cells, zinc-air batteries, and CO<sub>2</sub> electrolysis cells, demonstrating broad applicability for high-performance GDEs.","PeriodicalId":343,"journal":{"name":"Joule","volume":"5 1","pages":""},"PeriodicalIF":39.8,"publicationDate":"2025-11-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145478254","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Reversible solid oxide cells (RSOCs) represent a promising technology for efficient, long-term, and large-scale co-generation of power and fuel. However, commercializing RSOCs has been hindered by the inadequate electrocatalytic activity and stability of conventional oxygen (or air) electrode materials. In this work, we demonstrate that a high-entropy strategy effectively overcomes the classic activity-stability trade-off in perovskite-based air electrode materials. The developed Pr0.25Nd0.25Gd0.25Sm0.25Ba0.25La0.25Sr0.25Ca0.25Co2O5+δ (HE-PBC) air electrode exhibits exceptional electrocatalytic activity and stability under realistic operating conditions. When integrated into oxygen ion-conducting RSOCs, the HE-PBC electrode nearly doubles the cell performance compared with the conventional electrode while reducing the degradation rate by more than an order of magnitude. Furthermore, proton-conducting RSOCs with the HE-PBC electrode exhibit outstanding performance, achieving a peak power density of 1.13 W cm−2 in fuel cell mode and a current density of 2.56 A cm−2 at 1.3 V in electrolysis mode at 600°C while maintaining excellent stability for over 1,000 h.
可逆固体氧化物电池（rsoc）是一种很有前途的高效、长期和大规模热电联产技术。然而，由于传统氧（或空气）电极材料的电催化活性和稳定性不足，rsoc的商业化一直受到阻碍。在这项工作中，我们证明了高熵策略有效地克服了钙钛矿基空气电极材料中经典的活性-稳定性权衡。所研制的Pr0.25Nd0.25Gd0.25Sm0.25Ba0.25La0.25Sr0.25Ca0.25Co2O5+δ (HE-PBC)空气电极在实际操作条件下表现出优异的电催化活性和稳定性。当集成到氧离子导电rsoc中时，HE-PBC电极的电池性能几乎是传统电极的两倍，同时将降解率降低了一个数量级以上。此外，具有HE-PBC电极的质子导电rsoc表现出出色的性能，在燃料电池模式下实现了1.13 W cm - 2的峰值功率密度，在600°C电解模式下在1.3 V下实现了2.56 a cm - 2的电流密度，同时保持了1000小时以上的优异稳定性。
{"title":"Breaking the activity-stability trade-off with a high-entropy perovskite oxygen electrode for sustainable solid oxide cells","authors":"Yucun Zhou, Xueyu Hu, Weilin Zhang, Zheyu Luo, Yuechao Yao, Tongtong Li, Yong Ding, Yu Chen, Meilin Liu","doi":"10.1016/j.joule.2025.102198","DOIUrl":"https://doi.org/10.1016/j.joule.2025.102198","url":null,"abstract":"Reversible solid oxide cells (RSOCs) represent a promising technology for efficient, long-term, and large-scale co-generation of power and fuel. However, commercializing RSOCs has been hindered by the inadequate electrocatalytic activity and stability of conventional oxygen (or air) electrode materials. In this work, we demonstrate that a high-entropy strategy effectively overcomes the classic activity-stability trade-off in perovskite-based air electrode materials. The developed Pr<sub>0.25</sub>Nd<sub>0.25</sub>Gd<sub>0.25</sub>Sm<sub>0.25</sub>Ba<sub>0.25</sub>La<sub>0.25</sub>Sr<sub>0.25</sub>Ca<sub>0.25</sub>Co<sub>2</sub>O<sub>5+δ</sub> (HE-PBC) air electrode exhibits exceptional electrocatalytic activity and stability under realistic operating conditions. When integrated into oxygen ion-conducting RSOCs, the HE-PBC electrode nearly doubles the cell performance compared with the conventional electrode while reducing the degradation rate by more than an order of magnitude. Furthermore, proton-conducting RSOCs with the HE-PBC electrode exhibit outstanding performance, achieving a peak power density of 1.13 W cm<sup>−2</sup> in fuel cell mode and a current density of 2.56 A cm<sup>−2</sup> at 1.3 V in electrolysis mode at 600°C while maintaining excellent stability for over 1,000 h.","PeriodicalId":343,"journal":{"name":"Joule","volume":"140 1","pages":""},"PeriodicalIF":39.8,"publicationDate":"2025-11-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145478123","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-11-07DOI: 10.1016/j.joule.2025.102197
Yuge Feng, Yoon Park, Shaoyun Hao, Chang Qiu, Shoukun Zhang, Zhou Yu, Zhiwei Fang, Tanguy Terlier, Chase Sellers, Khalid Mateen, Frank Despinois, Moussa Kane, Sibani Lisa Biswal, Haotian Wang
Conventional lithium-ion (Li-ion) battery recycling technologies, including pyrometallurgy and hydrometallurgy, require elevated temperatures or substantial chemical input to smelt or leach solid battery materials for Li separation. In this work, we leveraged the intrinsic delithiation chemistry of battery cathode materials as a separation mechanism and devised the zero-gap membrane electrode assembly (MEA) reactor for sustainable, scalable, and cost-effective Li recovery from waste LiFePO4 (LFP) battery black mass (BM). Our strategy achieved an impressive Li extraction Faradaic efficiency of 96.4%, yielding high-purity lithium hydroxide (LiOH) (∼99.0 wt %), and reduced energy consumption to as low as 103 kJ/kgBM. A 20 cm2 MEA reactor demonstrated stable operation for 1,000 h, processing ∼57 g of LFP BM and maintaining an average Li recovery rate of 89.8%. Additionally, the MEA reactor can be adapted to a roll-to-roll fashion to produce 0.98 M LiOH and can be extended to other cathode materials such as LiMn2O4, LiNi0.5Mn0.3Co0.2O2, and hybrid cathode materials.
{"title":"A direct electrochemical Li recovery from spent Li-ion battery cathode for high-purity lithium hydroxide feedstock","authors":"Yuge Feng, Yoon Park, Shaoyun Hao, Chang Qiu, Shoukun Zhang, Zhou Yu, Zhiwei Fang, Tanguy Terlier, Chase Sellers, Khalid Mateen, Frank Despinois, Moussa Kane, Sibani Lisa Biswal, Haotian Wang","doi":"10.1016/j.joule.2025.102197","DOIUrl":"https://doi.org/10.1016/j.joule.2025.102197","url":null,"abstract":"Conventional lithium-ion (Li-ion) battery recycling technologies, including pyrometallurgy and hydrometallurgy, require elevated temperatures or substantial chemical input to smelt or leach solid battery materials for Li separation. In this work, we leveraged the intrinsic delithiation chemistry of battery cathode materials as a separation mechanism and devised the zero-gap membrane electrode assembly (MEA) reactor for sustainable, scalable, and cost-effective Li recovery from waste LiFePO<sub>4</sub> (LFP) battery black mass (BM). Our strategy achieved an impressive Li extraction Faradaic efficiency of 96.4%, yielding high-purity lithium hydroxide (LiOH) (∼99.0 wt %), and reduced energy consumption to as low as 103 kJ/kg<sub>BM</sub>. A 20 cm<sup>2</sup> MEA reactor demonstrated stable operation for 1,000 h, processing ∼57 g of LFP BM and maintaining an average Li recovery rate of 89.8%. Additionally, the MEA reactor can be adapted to a roll-to-roll fashion to produce 0.98 M LiOH and can be extended to other cathode materials such as LiMn<sub>2</sub>O<sub>4</sub>, LiNi<sub>0.5</sub>Mn<sub>0.3</sub>Co<sub>0.2</sub>O<sub>2</sub>, and hybrid cathode materials.","PeriodicalId":343,"journal":{"name":"Joule","volume":"1 1","pages":""},"PeriodicalIF":39.8,"publicationDate":"2025-11-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145455379","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-11-07DOI: 10.1016/j.joule.2025.102195
Do-Hyeon Kim, Young-Han Lee, Jeong-Myeong Yoon, Pugalenthiyar Thondaiman, Byung Chul Kim, In-Chul Choi, Jeong-Hee Choi, Ki-Joon Jeon, Cheol-Min Park
Silicon (Si) is an attractive high-capacity anode material for all-solid-state Li-ion batteries (ASSLIBs). However, significant volume change, low ionic/electronic conductivity, poor solid-electrolyte compatibility, and high stack pressure requirements limit its practical applications. To address these issues, we propose Li–Si compound anodes for ASSLIBs, selected based on formation energies predicted by density functional theory. Among the Li–Si compounds, Li7Si3 (Li2.33Si) exhibits the highest ionic conductivity along with high electronic conductivity, making it an ideal anode material. Moreover, its Li-storage mechanism (Li2.33 + αSi, 0 < α < 0.92) enables ultra-stable cycling with negligible volume change. A Li2.33Si|LiNi0.6Co0.2Mn0.2O2 full cell achieved high areal capacity, long cycle life, fast rate capability, wide operating temperature range, and low stack pressure, demonstrating that the Li2.33Si anode meets all the key requirements for high-performance anodes. Consequently, Li–Si compound anodes will serve as a key enabler for advancing ASSLIB technology, with the concept broadly extendable to other Li-based compounds.
{"title":"Li–Si compound anodes enabling high-performance all-solid-state Li-ion batteries","authors":"Do-Hyeon Kim, Young-Han Lee, Jeong-Myeong Yoon, Pugalenthiyar Thondaiman, Byung Chul Kim, In-Chul Choi, Jeong-Hee Choi, Ki-Joon Jeon, Cheol-Min Park","doi":"10.1016/j.joule.2025.102195","DOIUrl":"https://doi.org/10.1016/j.joule.2025.102195","url":null,"abstract":"Silicon (Si) is an attractive high-capacity anode material for all-solid-state Li-ion batteries (ASSLIBs). However, significant volume change, low ionic/electronic conductivity, poor solid-electrolyte compatibility, and high stack pressure requirements limit its practical applications. To address these issues, we propose Li–Si compound anodes for ASSLIBs, selected based on formation energies predicted by density functional theory. Among the Li–Si compounds, Li<sub>7</sub>Si<sub>3</sub> (Li<sub>2.33</sub>Si) exhibits the highest ionic conductivity along with high electronic conductivity, making it an ideal anode material. Moreover, its Li-storage mechanism (Li<sub>2.33 + α</sub>Si, 0 < α < 0.92) enables ultra-stable cycling with negligible volume change. A Li<sub>2.33</sub>Si|LiNi<sub>0.6</sub>Co<sub>0.2</sub>Mn<sub>0.2</sub>O<sub>2</sub> full cell achieved high areal capacity, long cycle life, fast rate capability, wide operating temperature range, and low stack pressure, demonstrating that the Li<sub>2.33</sub>Si anode meets all the key requirements for high-performance anodes. Consequently, Li–Si compound anodes will serve as a key enabler for advancing ASSLIB technology, with the concept broadly extendable to other Li-based compounds.","PeriodicalId":343,"journal":{"name":"Joule","volume":"127 1","pages":""},"PeriodicalIF":39.8,"publicationDate":"2025-11-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145455378","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-11-05DOI: 10.1016/j.joule.2025.102178
Chao-Yang Wang, Kaiqiang Qin, Nitesh Gupta
We examine the latest developments in all-climate batteries (ACBs) that enable efficient and resilient energy storage across extreme temperature ranges, e.g., from −50oC to +60oC. A figure of merit is presented to quantify where the current state of art, the latest advances and the future targets stand in this rapidly evolving field. We review two distinctive approaches driving power and stability improvements in both low- and high-temperature environments: materials innovation (particularly electrolyte formulations) and thermal actuation. It is found that there are still two-orders-of-magnitude gaps from the ACB target of high-temperature stability by materials innovation alone and that the material-thermal synergetic approach promises to attain the dual goals of ACBs for uncompromised power and stability at both low and high temperatures. Future research should be focused on developing heat-tolerant electrolytes and electrodes that can survive in 70oC–85oC environments.
{"title":"All-climate battery energy storage","authors":"Chao-Yang Wang, Kaiqiang Qin, Nitesh Gupta","doi":"10.1016/j.joule.2025.102178","DOIUrl":"https://doi.org/10.1016/j.joule.2025.102178","url":null,"abstract":"We examine the latest developments in all-climate batteries (ACBs) that enable efficient and resilient energy storage across extreme temperature ranges, e.g., from −50<sup>o</sup>C to +60<sup>o</sup>C. A figure of merit is presented to quantify where the current state of art, the latest advances and the future targets stand in this rapidly evolving field. We review two distinctive approaches driving power and stability improvements in both low- and high-temperature environments: materials innovation (particularly electrolyte formulations) and thermal actuation. It is found that there are still two-orders-of-magnitude gaps from the ACB target of high-temperature stability by materials innovation alone and that the material-thermal synergetic approach promises to attain the dual goals of ACBs for uncompromised power and stability at both low and high temperatures. Future research should be focused on developing heat-tolerant electrolytes and electrodes that can survive in 70<sup>o</sup>C–85<sup>o</sup>C environments.","PeriodicalId":343,"journal":{"name":"Joule","volume":"30 1","pages":""},"PeriodicalIF":39.8,"publicationDate":"2025-11-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145442074","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Solar distillation with backward-evaporating structures has recently exhibited promising freshwater-production performance and attractive application prospects for alleviating global water scarcity using solar energy. Although sustainably efficient distillation approaches have been developed, extensive potential still exists in its efficiency promotion and sustainable operation, and specific pathways need to be explored toward practical applications. In this perspective, we discuss the theoretical limits of solar-to-water energy conversion efficiency and identify key approaches to improve the distillation process. We reveal the underlying mechanism of salt-ion movement of current effective anti-salt-precipitation approaches, and we illustrate how to accelerate or inhibit salt removal through tailored driving-force combinations. In addition, we highlight the balance between brine discharge and energy efficiency under brine conditions for sustainable and efficient distillation. Toward a wide application level, we summarize the integrated applications of backward-evaporating solar distillation in energy-resource co-production. We also propose scalable water-production operation modes and indicate the realistic challenges for scaled-up deployment. Finally, we conduct an economic assessment and technology comparison with other solar thermal desalination technologies, and we propose a cost evaluation method for guiding multistage system design, aiming to move this technology forward to practical applications.
{"title":"Backward-evaporating solar distillation: From efficiency promotion to practical application","authors":"Ziye Zhu, Yanjie Zheng, Hongfei Zheng, Jianyin Xiong","doi":"10.1016/j.joule.2025.102193","DOIUrl":"https://doi.org/10.1016/j.joule.2025.102193","url":null,"abstract":"Solar distillation with backward-evaporating structures has recently exhibited promising freshwater-production performance and attractive application prospects for alleviating global water scarcity using solar energy. Although sustainably efficient distillation approaches have been developed, extensive potential still exists in its efficiency promotion and sustainable operation, and specific pathways need to be explored toward practical applications. In this perspective, we discuss the theoretical limits of solar-to-water energy conversion efficiency and identify key approaches to improve the distillation process. We reveal the underlying mechanism of salt-ion movement of current effective anti-salt-precipitation approaches, and we illustrate how to accelerate or inhibit salt removal through tailored driving-force combinations. In addition, we highlight the balance between brine discharge and energy efficiency under brine conditions for sustainable and efficient distillation. Toward a wide application level, we summarize the integrated applications of backward-evaporating solar distillation in energy-resource co-production. We also propose scalable water-production operation modes and indicate the realistic challenges for scaled-up deployment. Finally, we conduct an economic assessment and technology comparison with other solar thermal desalination technologies, and we propose a cost evaluation method for guiding multistage system design, aiming to move this technology forward to practical applications.","PeriodicalId":343,"journal":{"name":"Joule","volume":"166 1","pages":""},"PeriodicalIF":39.8,"publicationDate":"2025-11-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145442075","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-11-03DOI: 10.1016/j.joule.2025.102201
Huaian Zhao, Lizhi Xiang, Binghan Cui, Qingjie Zhou, Jiannan Du, Sai Li, Zheng Liu, Geping Yin, Guokang Han, Chunyu Du
Understanding how inhomogeneous reactions evolve across the battery electrode is essential for deciphering degradation mechanisms and improving the performance of commercial batteries. However, operando tracking of such dynamic processes remains challenging due to the lack of non-destructive techniques with spatiotemporal resolution. Here, we develop a magnetic field mapping technique that enables operando monitoring of reaction inhomogeneities across spatial and temporal dimensions. This approach reveals a self-regulating dynamic feedback mechanism, which provides a theoretical framework for interpreting the spatiotemporal evolution of inhomogeneous reactions under different C-rates, battery designs, and environmental conditions. This method identifies otherwise inaccessible design defects by directly resolving their spatially localized influence on reaction dynamics. It also directly visualizes mechanically induced reaction bottlenecks and the redirection of reaction pathways, offering new operando insights into mechano-electrochemical coupling in batteries. These findings provide a new approach for understanding inhomogeneous degradation, guiding electrode design, and advancing multi-dimensional diagnostic strategies for commercial batteries.
{"title":"Operando mapping of the dynamic evolution of spatially inhomogeneous reactions in commercial batteries","authors":"Huaian Zhao, Lizhi Xiang, Binghan Cui, Qingjie Zhou, Jiannan Du, Sai Li, Zheng Liu, Geping Yin, Guokang Han, Chunyu Du","doi":"10.1016/j.joule.2025.102201","DOIUrl":"https://doi.org/10.1016/j.joule.2025.102201","url":null,"abstract":"Understanding how inhomogeneous reactions evolve across the battery electrode is essential for deciphering degradation mechanisms and improving the performance of commercial batteries. However, operando tracking of such dynamic processes remains challenging due to the lack of non-destructive techniques with spatiotemporal resolution. Here, we develop a magnetic field mapping technique that enables operando monitoring of reaction inhomogeneities across spatial and temporal dimensions. This approach reveals a self-regulating dynamic feedback mechanism, which provides a theoretical framework for interpreting the spatiotemporal evolution of inhomogeneous reactions under different C-rates, battery designs, and environmental conditions. This method identifies otherwise inaccessible design defects by directly resolving their spatially localized influence on reaction dynamics. It also directly visualizes mechanically induced reaction bottlenecks and the redirection of reaction pathways, offering new operando insights into mechano-electrochemical coupling in batteries. These findings provide a new approach for understanding inhomogeneous degradation, guiding electrode design, and advancing multi-dimensional diagnostic strategies for commercial batteries.","PeriodicalId":343,"journal":{"name":"Joule","volume":"27 1","pages":""},"PeriodicalIF":39.8,"publicationDate":"2025-11-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145428016","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-11-03DOI: 10.1016/j.joule.2025.102177
Ruqing Fang, Junning Jiao, Wei Li, Royal C. Ihuaenyi, Martin Z. Bazant, Juner Zhu
We introduce mechano-electrochemical impedance spectroscopy (MEIS) as a technique that complements electrochemical impedance spectroscopy (EIS) by probing coupled mechanical-electrochemical dynamics in batteries. MEIS leverages electrode expansion and contraction during ion intercalation, which induces measurable pressure fluctuations under mechanical constraint. By applying a small sinusoidal current and recording the pressure response, MEIS defines its spectrum as the frequency-domain ratio of pressure to current. Experiments across multiple chemistries reveal distinct MEIS features that depend strongly on state of charge (SOC) and are sensitive to state of health (SOH), underscoring its diagnostic potential. An idealized analytical model links semicircles to mechanical stiffness and vertical features to intercalation-induced pseudo-damping, while a porous-electrode model incorporating a poro-viscoelastic bridge explains counterintuitive behaviors such as phase reversals and quadrant shifts. By connecting particle-scale deformation to electrode-level responses, MEIS opens new avenues for SOC estimation, degradation analysis, and health diagnostics in energy storage systems.
{"title":"Mechano-electrochemical impedance spectroscopy: Experimentation, interpretation, and application","authors":"Ruqing Fang, Junning Jiao, Wei Li, Royal C. Ihuaenyi, Martin Z. Bazant, Juner Zhu","doi":"10.1016/j.joule.2025.102177","DOIUrl":"https://doi.org/10.1016/j.joule.2025.102177","url":null,"abstract":"We introduce mechano-electrochemical impedance spectroscopy (MEIS) as a technique that complements electrochemical impedance spectroscopy (EIS) by probing coupled mechanical-electrochemical dynamics in batteries. MEIS leverages electrode expansion and contraction during ion intercalation, which induces measurable pressure fluctuations under mechanical constraint. By applying a small sinusoidal current and recording the pressure response, MEIS defines its spectrum as the frequency-domain ratio of pressure to current. Experiments across multiple chemistries reveal distinct MEIS features that depend strongly on state of charge (SOC) and are sensitive to state of health (SOH), underscoring its diagnostic potential. An idealized analytical model links semicircles to mechanical stiffness and vertical features to intercalation-induced pseudo-damping, while a porous-electrode model incorporating a poro-viscoelastic bridge explains counterintuitive behaviors such as phase reversals and quadrant shifts. By connecting particle-scale deformation to electrode-level responses, MEIS opens new avenues for SOC estimation, degradation analysis, and health diagnostics in energy storage systems.","PeriodicalId":343,"journal":{"name":"Joule","volume":"85 1","pages":""},"PeriodicalIF":39.8,"publicationDate":"2025-11-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145427863","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
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